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Solar-Driven Lignin Oxidation via Hydrogen Atom Transfer with a Dye-Sensitized TiO2 Photoanode
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-02-17 , DOI: 10.1021/acsenergylett.9b02391
Shuya Li 1 , Zhi-Jun Li 2 , Hyun Yu 1 , Marion Ryan Sytu 1 , Yunxuan Wang 3 , Debora Beeri 4 , Weiwei Zheng 2 , Benjamin D. Sherman 4 , Chang Geun Yoo 3 , Gyu Leem 1, 5
Affiliation  

Molecular-based dye-sensitized photoelectrochemical cells (DSPECs) have traditionally targeted solar-driven water splitting for the conversion of solar energy into fuels in aqueous media. This work reports the use of a DSPEC-type photoanode specifically designed to carry out chemoselective oxidation of benzylic alcohol moieties in lignin model compounds and real lignin in organic media. The TiO2-based photoanode incorporates a surface-bound Ru(II)-based photocatalyst and solution-dissolved hydrogen atom transfer (HAT) co-catalyst to perform solar-driven photocatalytic oxidation of the lignin substrates. Under aerobic conditions with simulated solar illumination, conversion efficiencies in excess of 90% are observed for the formation of the oxidized ketone product from model compounds. The DSPEC half-cell exhibited impressive long-term durability, sustaining photocatalytic oxidation of the lignin model compound over a net illumination period of 80 h. This photoelectrochemical heterogeneous catalytic process provides a unique foundation to perform selective C–O bond cleavage for real lignin conversion technologies.

中文翻译:

染料敏化的TiO 2光电阳极通过氢原子转移进行太阳驱动的木质素氧化

传统上,基于分子的染料敏化光电化学电池(DSPEC)的目标是太阳能驱动的水分解,用于将太阳能转化为水性介质中的燃料。这项工作报告了DSPEC型光阳极的使用,该光阳极专门设计用于对木质素模型化合物中的苄醇部分和有机介质中的实际木质素进行化学选择性氧化。TiO 2的光阳极结合了基于表面结合Ru(II)的光催化剂和溶液溶解的氢原子转移(HAT)助催化剂,以进行木质素基质的太阳能驱动光催化氧化。在模拟太阳光照下的有氧条件下,观察到从模型化合物形成氧化酮产物的转化效率超过90%。DSPEC半电池表现出令人印象深刻的长期耐用性,在80 h的净光照时间内维持木质素模型化合物的光催化氧化。这种光电化学非均相催化过程为进行真正的木质素转化技术进行选择性的C–O键裂解提供了独特的基础。
更新日期:2020-02-17
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